Ammonium deficiency caused by heterogeneous reactions during a super Asian dust episode

Mineral dust particles exert profound impacts on air quality, visibility, and ocean biogeochemistry. Interactions between dust particles and other anthropogenic pollutants modify not only the size spectrum and morphology but also physicochemical properties of dust particles, thereby affecting their radiative properties and ability to act as cloud condensation nuclei and in turn their impact on climate. Here we report field observations on the surface chemical transformations in a super Asian dust plume captured in coastal areas of China and the adjacent marginal seas. The dust plume showed enhanced concentrations of sulfate, nitrate, and calcium along with a decrease in ammonium. The percentages of total Ca in water-soluble form increased from an intrinsic value of similar to 5% to 25-40% at four stations along the path of the dust plume. From these increases, we estimated the extent to which carbonate was modified by heterogeneous reactions and calculated that the enhanced sulfate and nitrate could account for 40-60% of the observed concentrations. Our observation suggests that the formation of ammonium sulfate via the H2SO4-NH3-H2O ternary system was impeded by heterogeneous reactions in the marine boundary layer when dust loads exceeded a certain threshold. A conceptual model is proposed to elucidate the heterogeneous reactions during the super Asian dust event and their impacts on atmospheric chemistry.